Panagiota Tsetsakos


Summary of Journal Article



Title: Addition of Nitryl Iodide to Olefins

A. Hassner, J.E. Kropp, G.J. Kent, J. Org. Chem.,1969, 34, 2628- 2632



http://dx.doi.org/10.1021/jo01261a030



  • Birchenbach first reported the reaction of silver nitrate and iodine with cyclohexene to give nitro and iodo-nitro adducts, but was disregarded until many years later
  • Nitryl iodide reaction has been used in the nitration of sugars
  • Silver nitrate with iodine would lead to INO2 that can be cleaved heterolytically ( such as I+ NO2-) or homolytically (production of free radicals)
  • Information about the stereochemistry of the addition of INO2, was obtained by reaction silver nitrate and iodine with 2-cholestene in ether
  • NMR data shows that iodine has a very strong anisotropic effect (C-19 methyl signal was at 8.83 ppm)
  • Anisotropic effect increases from chlorine to bromine to iodine
  • The nitro group in adduct 1 occupied the 3a site, that suggested that pseudohalogen was reacting as INO2 but as NO2I.
  • This was further supported by the regiochemistry of the reaction of silver nitrate and iodine with styrene
  • t-butyethylene was treated with silver nitrate and iodine and gave compound 11
  • Furthermore HI was eliminated leading to compound 12, a vinyl nitro
  • Reduction of compound 12 with NaBH4 gave compound 13, a saturated nitro compound
  • Adduct 1 was refluxed with silver nitrate in alcohol only a small amount of the nitro alkene was made, but when 1 was refluxed in methanol and silver oxide, 3-nitro-2-cholestene was formed in 99% yield
  • To further prove that NO2I forms, the solids created from the reaction of the silver nitrate with iodine were removed before the addition of the alkene
  • When 2-cholestene was added, 1 was formed but in a very poor yield
  • Dinitrogen tetroxide was added slowly to a 2-cholestene and iodine solution in nonpolar solvents; the end result was compound 1
  • Trans stereochemistry was observed suggesting that a stable pyramidal radical is formed or that quenching with iodine is a lot faster than inversion of the radical formed.
  • It is suggested that the nitroalklyl radical denoted as 1a becomes trapped quickly and efficiently by iodine and is then converted to compound denoted as 1b that furthermore supports the formation of a product that is kinetically controlled and also not favored sterically.
  • NO2I was added to both cis and trans stilbene; the product was a diastereoisomeric mixture
  • After NO2I was added to excess cis- stilbene, NMR data showed that unreacted stilbene in the crude product was only the cis isomer.
  • This was strong evidence that the nitro radical formation was irreversible
  • NO2I when reacted with toluene and methyl benzoate did not lead to any nitration suggesting that NO2I is not a good source of nitrylium ions
  • The remainder of the article was the experimental section that described all the experimental procedures.